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These are major spoilers.. Unless you have watched the anime, it may not be a good idea to read them.

Spoiler for D. Gray-Man:

I dropped D. Gray-Man after watching 70+ episodes and completed Darker than Black. Both series are action animes that feature supernatural elements. However, D. Gray-Man has quite some obvious underlying politics to it. Generally, it starts off as quite a good shounen supernatural anime but after 40+ episodes, the story turn into politics. It is generally about the government of Japan being evil as that they are manipulated by demons and that the main characters led by Allen Walker had to invite some friends from an Oriental nation to help them fight these demons. The Oriental nation is the hometown of the female lead, Lenalee and also Panda-sensei who trains Levi. By that point, the story was no longer interesting as that it is no longer a supernatural shounen anime. It is quite a pity considering that the battles between the exorcists and the demons were pretty intense and awesome, yet..

Spoiler for Darker than Black:

The story is pretty much about the Chinese and the foreigners wrecking havoc in Japan. Generally, all the characters have supernatural abilities and are on some sort of agenda. The story is average, the battles are pretty good but the ending is rather incomplete. Its like there is no ending, yet there is one.

If you have to watch one of the two, I would suggest Darker than Black as that Nana-sama voices one of the main characters.

D. Gray Man is shounen, so it has a lot of action, but also it's darker than most other shounens out there, which gives it a little edge. However, it has issues with pacing, inconsistent animation and fillers.

Darker than Black has definitely better production quality - music, animation, story, but the ending was kind of mediocre. A second season is coming up, though, so you might give it a try.

Darker than black is getting a 2nd season I think, I haven't seen it but I'd guess it's better than D.Gray-man in terms of seriousness...but when(/if) D.Gray-man gets another season, it will definitely have the upper hand on the psychological domain. Hmm...toss a coin?

Skip D.Gray Man. It's very much like Naurto which isn't bad per say, but the pacing and fillers are what killed both series for me even though I found both storylines to be quite facinating. Had D.Gray Man and Naurto just stuck with the main plot and avoided the pointless fillers and the 5 episode long fights then they would have been so much better off even if it meant that they were only half as long.

Well if you want something along lines of CG I would say skip both these shows . They are different, something along lines of CG minus mecha would Death-Note or Monster.

If I were to make a direct comparison I would say DTB is better than DGM . If I were to properly compare both these shows I would say DGM . The reason being a well scripted anime cant be compared with a long running weekly manga . The question you should be asking yourself before choosing would be

* Do you have time on your hands ?

Spoiler for Anime:

- DTB spans 25 + Ep while DGM 103 Epsiodes

* Do you mind manga ?

Spoiler for Anime:

- AS DGM anime season is over so continuity is only found in the manga

- While DTB is renewed for a second season this fall/winter

* What type of anime shows Do you prefer ?

Spoiler for Anime:

- DTB is a dark themed show which deals with relationships. While DGM is a light hearted show with ample amounts of tense moments .

If time is not a problem I would say watch both these shows they are quite enjoyable and entertaining